▎ 摘　　要

The integration of electronic components and the popularity of flexible devices have come up with higher expectations for the heat dissipation capability and comprehensive mechanical performance of thermal management materials. In this work, after the modification of polyimide (PI) fibers through oxidation and amination, the obtained PDA@OPI fibers (polydopamine (PDA)-modified pre-oxidized PI fibers) with abundant amino groups were mixed into graphene oxide (GO) to form uniform GO-PDA@OPI composites. Followed by evaporation, carbonization, graphitization and mechanical compaction, the G-gPDA@OPI films with a stable three-dimensional (3D) long-range interconnected covalent structure were built. In particular, due to the rich covalent bonds between GO layers and PDI@OPI fibers, the enhanced synergistic graphitization promotes an ordered graphitized structure with less interlayer distance between adjacent graphene sheets in composite film. As a result, the optimized G-gPDA@OPI film displays an improved tensile strength of 78.5 MPa, tensile strain of 19.4% and thermal conductivity of 1028 W/(m center dot K). Simultaneously, it also shows superior flexibility and high resilience. This work provides an easily-controlled and relatively low-cost route for fabricating multifunctional graphene heat dissipation films.